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Electronic-property dependent interactions between tetracycline and graphene nanomaterials in aqueous solution

Journal of Environmental Sciences 2018年第4期30卷 286-294页

作者： Lin He Fei-fei Liu Mengyao Zhao Zhen Qi Xuefei Sun Muhammad Zaheer Afzal Xiaomin Sun Yanhui Li Jingcheng Hao Shuguang Wang Shandong Key Laboratory of Water Pollution Control and Resource Reuse School of Environmental Science and EngineeringShandong University Insistute of Marine Science and Technology Shandong University Environment Research Institute Shandong University Laboratory of Fiber Materials and Modern Textile The Growing Base for State Key Laboratory Qingdao University Key Laboratory of Colloid and Interface Chemistry Ministry of Education Shandong University

Understanding the interactions between graphene nanomaterials（GNMs） and antibiotics in aqueous solution is critical to both the engineering applications of GNMs and the assessment of their potential impact on the fate and transport of antibiotics in the aquatic environment. In this study, adsorption of one common antibiotic, tetracycline, by graphene oxide（GO） and reduced graphene oxide（RGO） was examined with multi-walled carbon nanotubes（MWCNTs） and graphite as comparison. The results showed that the tetracycline adsorption capacity by the four selected carbonaceous materials on the unit mass basis followed an order of GO ＆gt; RGO ＆gt; MWCNTs ＆gt; graphite. Upon normalization by surface area,graphite, RGO and MWCNTs had almost the same high tetracycline adsorption affinity while GO exhibited the lowest. We proposed π-electron-property dependent interaction mechanisms to explain the observed different adsorption behaviors. Density functional theory（DFT） calculations suggested that the oxygen-containing functional groups on GO surface reduced its π-electron-donating ability, and thus decreased the π-based interactions between tetracycline and GO surface. Comparison of adsorption efficiency at different p H indicated that electrostatic interaction also played an important role in tetracycline-GO interactions. Site energy analysis confirmed a highly heterogeneous distribution of the binding sites and strong tetracycline binding affinity of GO surface.

关键词： Graphene oxide Reduced graphene oxide Tetracycline Adsorption DFT calculation π-Based interaction

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Overturned Loading of Inert CeO2to Active Co3O4for Unusually Improved Catalytic Activity in Fenton-Like Reactions

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Angewandte Chemie 2022年第16期134卷

作者： Chunli Song Qing Zhan Dr. Fei Liu Chuan Wang Dr. Hongchao Li Xuan Wang Prof. Xuefeng Guo Prof. Yingchun Cheng Wei Sun Prof. Li Wang Prof. Jieshu Qian Prof. Bingcai Pan Jiangsu Key Laboratory of Chemical Pollution Control and Resources Reuse School of Environmental and Biological Engineering Nanjing University of Science and Technology 200 Xiao Ling Wei Nanjing 210094 China Key Laboratory of Flexible Electronics & Institute of Advanced Materials Jiangsu National Synergetic Innovation Center for Advanced Materials Nanjing Tech University Nanjing 211816 China Key Lab of Mesoscopic Chemistry MOE School of Chemistry & Chemical Engineering Nanjing University Nanjing 210023 China Key Laboratory of Catalysis and Energy Materials Chemistry of Ministry of Education South-Central University for Nationalities Wuhan 430074 China Research Center for Environmental Nanotechnology (ReCENT) School of Environment State Key Laboratory of Environmental Pollution and Resources Reuse Nanjing University Nanjing 210023 China

In the past decades, numerous efforts have been devoted to improving the catalytic activity of nanocomposites by either exposing more active sites or regulating the interaction between the support and nanoparticles while keeping the structure of the active sites unchanged. Here, we report the fabrication of a Co 3 O 4 −CeO 2 nanocomposite via overturning the loading direction, i.e., loading an inert CeO 2 support onto active Co 3 O 4 nanoparticles. The resultant catalyst exhibits unexpectedly higher activity and stability in peroxymonosulfate-based Fenton-like reactions than its analog prepared by the traditional impregnation method. Abundant oxygen vacancies (O v with a Co⋅⋅⋅O v ⋅⋅⋅Ce structure instead of Co⋅⋅⋅O v ) are generated as new active sites to facilitate the cleavage of the peroxide bond to produce SO 4 .− and accelerate the rate-limiting step, i.e., the desorption of SO 4 .− , affording improved activity. This strategy is a new direction for boosting the catalytic activity of nanocomposite catalysts in various scenarios, including environmental remediation and energy applications.

关键词： CO Oxidation Fenton-Like Reaction Nanocomposite Catalyst Overturned Loading Oxygen Vacancy

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Ketyl Radical Anion Mediated Radical Polymerization and Anionic Ring-Opening Polymerization to Give Polymers with Low Molecular Weight Distribution

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Angewandte Chemie 2023年第31期135卷

作者： Yu-Jiao Chen Liang-Tao Wu Tai-An Li Meng-Qin Pu Prof. Xiao-Li Sun Prof. Hongli Bao Prof. Wen-Ming Wan College of Environment and Resources Engineering Research Center of Polymer Green Recycling of Ministry of Education Fujian Key Laboratory of Pollution Control & Resource Reuse Fujian Normal University Fuzhou 350007 P. R. China Key Laboratory of Coal to Ethylene Glycol and Its Related Technology State Key Laboratory of Structural Chemistry Center for Excellence in Molecular Synthesis Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou 350002 P. R. China College of Chemistry and Materials Science Fujian Normal University Fuzhou 350007 P. R. China

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Frontispiece: A Showcase of Green Chemistry: Sustainable Synthetic Approach of Zirconium-Based MOF Materials

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Chemistry – A European Journal 2021年第39期27卷

作者： Jiarui Fu Dr. Yi-nan Wu College of Environmental Science and Engineering State Key Laboratory of Pollution Control and Resource Reuse Tongji University Siping Rd 1239 200092 Shanghai P.R. China Shanghai Institute of Pollution Control and Ecological Security Siping Rd 1239 200092 Shanghai P.R. China

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Improving The Biodegradability of Rice Straw by Electrochemical Pretreatment

SSRN

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SSRN 2022年

作者： Sun, Shaohua Zhang, Yuanyuan Yang, Zhaoyang Liu, Chunmei Zuo, Xiaoyu Tang, Yang Wan, Pingyu Liu, Yanping Li, Xiujin Coulon, Frederic Hu, Qing Yang, Xiao Jin State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical Technology 15 Beisanhuan East Road Chaoyang District Beijing100029 China Beijing City Environmental Pollution Control and Resource Reuse Engineering Center Beijing University of Chemical Technology 15 Beisanhuan East Road Chaoyang District Beijing100029 China National Fundamental Research Laboratory of New Hazardous Chemicals Assessment and Accident Analysis Beijing University of Chemical Technology Beijing100029 China School of Water Energy and Environment Cranfield University Cranfield MK43 0AL United Kingdom School of Environmental Science and Engineering South University of Science and Technology Guangdong Shenzhen518055 China Beijing Huanding Environmental Big Data Institute No. 1 Wangzhuang Road Beijing100083 China

In this study, the efficacy of three different pretreatments of rice straw including alkaline hydrogen peroxide (NaOH-H2O2), electrochemically produced NaOH-H2O2 (eNaOH-H2O2) and electrohydrolysis (EH) was investigated. All three pretreatments allowed to reach 80% of total biogas production within 23 and 25 days which was 3 to 5 days faster compared to conventional NaOH pretreatment. The cumulative biogas production was enhanced by 8%, 22% and 14% for NaOH-H2O2, eNaOH-H2O2 and EH, respectively compared to traditional treatment. The eNaOH-H2O2 pretreatment decreased the crystallinity of cellulose and created a porous surface vein, thus promoting microbial degradation of lignocellulose. The findings of this study demonstrate that electrochemical pretreatment provides a promising approach for efficiently utilizing rice straw biomass to produce renewable electricity. © 2022, The Authors. All rights reserved.

关键词： Oxidation

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Enhanced debromination of 4-bromophenol by the UV/sulfite process：Efficiency and mechanism

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Journal of Environmental Sciences 2017年第4期29卷 231-238页

作者： Bihuang Xie Xuchun Li Xianfeng Huang Zhe Xu Weiming Zhang Bingcai Pan State Key Laboratory of Pollution Control and Resource Reuse School of the EnvironmentNanjing University

Halogenated aromatic compounds have attracted increasing concerns due to their toxicity and persistency in the environment, and dehalogenation is one of the promising treatment and detoxification methods. Herein, we systematically studied the debromination efficiency and mechanism of para-bromophenol（4-BP） by a recently developed UV/sulfite process. 4-BP underwent rapid degradation with the kinetics accelerated with the increasing sulfite concentration, pH（6.1–10） and temperature, whereas inhibited by dissolved oxygen and organic solvents. The apparent activation energy was estimated to be 27.8 kJ/mol. The degradation mechanism and pathways of 4-BP were explored by employing N2O and nitrate as the electron scavengers and liquid chromatography/mass spectrometry to identify the intermediates. 4-BP degradation proceeded via at least two pathways including direct photolysis and hydrated electron-induced debromination. The contributions of both pathways were distinguished by quantifying the quantum yields of 4-BP via direct photolysis and hydrated electron production in the system. 4-BP could be readily completely debrominated with all the substituted Br released as Br-, and the degradation pathways were also proposed. This study would shed new light on the efficient dehalogenation of brominated aromatics by using the UV/sulfite process.

关键词： Debromination Brominated aromatics UV/sulfite process Hydrated electron Mechanism

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Phytotoxicity and groundwater impacts of leaching from thermal treatment residues in roadways

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Journal of Environmental Sciences 2018年第1期30卷 58-67页

作者： Khamphe Phoungthong Li-Ming Shao Pin-Jing He Hua Zhang State Key Laboratory of Pollution Control & Resource Reuse Tongji University Institute of Waste Treatment and Reclamation Tongji University Centre for the Technology Research and Training on Household Waste in Small Towns & Rural Area Ministry of Housing and Urban-Rural Development of PR China (MOHURD)

The use of coal fly ash（CFA）, municipal solid waste incinerator bottom ash（MSWIBA） and flue gas desulfurization residue（FGDR） in road construction has become very common owing to its economical advantages. However, these residues may contain toxic constituents that pose an environmental risk if they leach out and flow through the soil, surface water and ***, it is necessary to assess the ecotoxicity and groundwater impact of these residues before decisions can be made regarding their utilization for road construction. In this study,the physico-chemical characteristics, leaching and phytotoxicity of these residues were investigated. Specifically, multivariate analyses were used to evaluate the contributions of the leaching constituents of the CFA, MSWIBA and FGDR leachates to the germination index of wheat seeds. B, Ba, Cr, Cu, Fe and Pb were found to be more toxic to the wheat seeds than the other heavy metals. Furthermore, the leached concentrations of the constituents from the CFA, MSWIBA and FGDR were below the regulatory threshold limits of the Chinese identification standard for hazardous wastes. Analyses conducted using a numerical groundwater model（Wisc LEACH） indicated that the predicted field concentrations of metals from the CFA, MSWIBA and FGDR increased with time up to about 30 years at the point of compliance, then decreased with time and distance. Overall, this study demonstrated that the risks resulting from MSWIBA, CFA and FGDR leaching could be assessed before its utilization for road construction, providing crucial information for the adoption of these alternative materials.

关键词： Thermal treatment residues Bottom ash Flue gas desulfurization residue Heavy metals Phytotoxicity Groundwater impact

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In-situ heat-activated peroxymonosulfate pretreatment for effective biofouling mitigation strategies in seawater membrane distillation

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Desalination 2025年

作者： Jaewon Lee M. Obaid Najat A. Amin Weilong Yang Jieun Kim Taegeun Park Seonkyu Lee Seunghwan Woo Youngjin Kim Min Zhan Noreddine Ghaffour Seungkwan Hong Department of Civil Environmental and Architectural Engineering Korea University 145 Anam-ro Seongbuk-gu Seoul 02841 Republic of Korea Environmental Science and Engineering Division of Biological and Environmental Science and Engineering (BESE) King Abdullah University of Science and Technology (KAUST) Thuwal 23955-6900 Saudi Arabia China State Key Laboratory of Pollution Control and Resources Reuse School of Environment Nanjing University Nanjing 210023 China Department of Environmental Engineering Korea University 2511 Sejong-ro Sejong-si 30019 Republic of Korea

This study introduces an innovative in-situ heat-activated peroxymonosulfate (PMS) system as an efficient pretreatment strategy for mitigating biofouling in membrane distillation (MD) for seawater desalination. The system demonstrated robust microorganism inactivation in Red Sea seawater at MD operating temperatures of 60, 70, and 80 °C. This was attributed to the thermally accelerated generation of reactive chlorine species, achieving a log removal exceeding 3.6. The heat-activated PMS system significantly reduced the normalized vapor flux decline, by approximately 3.2 times at 60 °C (54 % vs. 17 %), 3.8 times at 70 °C (42 % vs. 11 %), and 5.7 times at 80 °C (56 % vs. 9.9 %), at a volume concentration factor of 4, compared to untreated system. These improvements were validated by optical coherence tomography imaging, which confirmed suppressed biofilm formation on the MD membrane surface, and live cell analysis, confirming a substantial decrease in live bacterial cell deposition. These findings highlight the potential of the heat-activated PMS system as a sustainable and efficient in-situ pretreatment strategy capable of addressing biofouling challenges and enhancing MD performance, offering a practical and scalable solution for seawater desalination applications.

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Exclusive microbially driven autotrophic iron-dependent denitrification in a reactor inoculated with activated sludge

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Water Research 2020年第0期170卷 115300-000页

作者： Tian, Tian Zhou, Ke Xuan, Liang Zhang, Jing-Xiao Li, Yu-Sheng Liu, Dong-Feng Yu, Han-Qing CAS Key Laboratory of Urban Pollutant Conversion Department of Applied Chemistry University of Science and Technology of China Hefei 230026 China School of Resources & Environmental Engineering Hefei University of Technology Hefei 230009 China School of Environmental Science & Engineering State Key Laboratory of Pollution Control and Resource Reuse Tongji University Shanghai 200092 China

Autotrophic iron-dependent denitrification (AIDD) is arising as a promising process for nitrogen removal from wastewater with a low carbon to nitrogen ratio. However, there is still a debate about the existence of such a process in activated sludge systems. This work provides evidence and elucidated the feasibility of autotrophic Fe(II)-oxidizing nitrate-reducing culture for nitrogen removal by long-term reactor operation, batch experimental verification, unstructured kinetic modeling and microbial community analyses. A relatively stable nitrate removal rate was achieved coupled with the oxidation of ferrous ions in 3-month operation of reactor. The kinetic modeling suggests that the iron oxidation was a growth-associated process in AIDD. Utilization of extracellular polymeric substances (and/or soluble microbial products) as electron donor for denitrification by heterotrophic denitrifiers was not mainly responsible for nitrogen removal in the reactor. After long-term operation of the reactor with activated sludge as inoculum, the enrichment culture KS-like consortium, dominated by Fe(II) oxidizer, Gallionellaceae, was successfully acclimated for autotrophic Fe(II)-oxidizing nitrate reduction. This work extents our understanding about the existence of such an autotrophic Fe(II)-oxidizing nitrate-reducing culture in both natural and engineered systems, and opens a door for its potential application in wastewater treatment. © 2019 Elsevier Ltd

关键词： Activated sludge Autotrophic iron-dependent denitrification (AIDD) Gallionellaceae Kinetic modeling Wastewater treatment

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Engineering carbon-encapsulated iron selenide with tunable inner voids for highly reversible conversion-reaction anodes

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Chemical Engineering Journal 2025年 519卷

作者： Nadeem Hussain Mehwish Kiran Zongyan Gao Zhu Zhu Shijing Luo Faxue Lu Junjian Li Xuechun Lou Lina Zhou Biqiong Chen Zuofeng Chen Tao Liu Shanghai Key Laboratory of Chemical Assessment and Sustainability School of Chemical Science and Engineering Tongji University No. 1239 Siping Road Shanghai 200092 PR China School of Materials Science and Engineering Anhui University Hefei 230601 PR China State Key Laboratory of Pollution Control and Resources Reuse College of Environmental Science and Engineering Tongji University 1239 Siping Road Shanghai 200092 PR China College of Materials Science and Engineering Sichuan University Chengdu Sichuan PR China School of Mechanical and Aerospace Engineering Queen's University Belfast Stranmillis Road Belfast BT9 5Ah United Kingdom.

Transition-metal selenides are promising anode materials for high-energy lithium-ion batteries due to their high theoretical capacity. However, enabling a highly reversible conversion reaction in these materials remains a significant challenge due to large volume fluctuations and poor electrical conductivity, which leads to structural degradation and sluggish reaction kinetics. To address these issues, we design a hollow-structured carbon-encapsulated iron selenide (FSC) via a simple, template-free solvothermal strategy. The internal void space within the hollow FeSe effectively accommodates volumetric expansion, preserving structural integrity during cycling, while the N-doped carbon shell enhances electrical conductivity and mitigates particle agglomeration. As a result, the FSC anode exhibits excellent lithium storage properties, including a high reversible capacity of 1054 mAh g −1 after 300 cycles at 0.1 A g −1 , an impressive rate capability up to 10 A g −1 (~10 mA cm −2 ), and outstanding long-term cycling stability over 1000 cycles at 1 A g −1 . Experimental characterization combined with density functional theory (DFT) calculations reveals a phase transition from hexagonal-FeSe to tetragonal-FeSe after the first activation cycle, favoring a highly reversible conversion reaction mechanism. This work provides a scalable strategy for designing structurally robust metal selenide anodes and offers fundamental insights into improving their electrochemical performance for next-generation lithium-ion batteries.

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